arXiv subjects

N. Büttgen

Publications and source records attributed to N. Büttgen.

At least 19 recordsLinked to original sources

arXiv2026

Novel Quantum Spin Liquid States in the $S = {\frac{1}{2}}$ Three-Dimensional Compound Y$_{3}$Cu$_{2}$Sb$_{3}$O$_{14}$

The three-dimensional $S = {\frac{1}{2}}$ system Y$_{3}$Cu$_{2}$Sb$_{3}$O$_{14}$ consists of two inequivalent Cu$^{2+}$ sites, each forming an edge shared triangular lattice. Our magnetic susceptibility $χ(T)$, specific heat $C_p(T)$, $^{89}$Y nuclear magnetic resonance (NMR), muon spin relaxation ($\upmu\mathrm{SR}$), and electron spin resonance (ESR) measurements on this system confirm the absence of any long-range magnetic ordering and the persistence of spin dynamics down to 0.077 K. In $^{89}$Y NMR we find an anomaly at about 120 K which we suggest arises from a fraction of the spins condensing into a singlet (a valence bond solid VBS) state. A plateau in the muon relaxation rate is observed between 60 K and 10 K (signifying the VBS state from a fraction of the spins) followed by an increase and another plateau below about 1 K (presumably signifying the quantum spin liquid state from all the spins). Our density functional theory calculations find a dominant antiferromagnetic interaction along the body diagonal with inequivalent Cu(1) and Cu(2) ions alternately occupying the corners of the cube. All other near-neighbour interactions between the Cu ions are also found to be antiferromagnetic and are thought to drive the frustration.

cond-mat.str-el↗

arXiv2026

Observation of a gapped phase in the one-dimensional $S = {\frac{1}{2}}$ Heisenberg antiferromagnetic chain Cu(Ampy)ClBr

Spin-1/2 Heisenberg antiferromagnetic frustrated spin chain systems display exotic ground states with unconventional excitations and distinct quantum phase transitions as the ratio of next-nearest-neighbor to nearest-neighbor coupling is tuned. We present a comprehensive investigation of the structural, magnetic, and thermodynamics properties of the spin-1/2 compound, Cu(Ampy)ClBr (Ampy= C$_6$H$_8$N$_2$ = 2-(Aminomethyl)pyridine) via x-ray diffraction, magnetization, specific heat, $^1$H nuclear magnetic resonance (NMR), electron spin resonance (ESR), and muon spin relaxation ($μ$SR) techniques. The crystal structure features an anisotropic triangular chain lattice of magnetic Cu$^{2+}$ ions. Our bulk and local probe experiments detect neither long-range magnetic ordering nor spin freezing down to 0.06 K despite the presence of moderate antiferromagnetic interaction between Cu$^{2+}$ spins as reflected by a Curie-Weiss temperature of about $-9$ K from the bulk susceptibility data. A broad maximum is observed at about 9 K in magnetic susceptibility and specific heat data, indicating the onset of short-range spin correlations. At low temperatures, the zero-field magnetic specific heat and the $^1$H NMR spin-lattice relaxation rate follow an exponential temperature dependence, indicating the presence of gapped magnetic excitations. Furthermore, persistent spin dynamics down to 0.088 K observed by zero-field $μ$SR evidences lack of any static magnetism.

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arXiv2021

Failure to achieve the $J_{eff}$~=~0 state even in nearly isolated Ir$^{5+}$ in Sr$_3$NaIrO$_6$: are iridates enough for realizing true $j$-$j$ coupling?

Spin-orbit coupling (SOC) often gives rise to interesting electronic and magnetic phases in an otherwise ordinary pool of paramagnetic heavy metal oxides. In presence of strong SOC, assumed to be working in $j$-$j$ coupling regime, 5$d^4$ iridates are generally speculated to possess a nonmagnetic $J_{eff}$~=~0 singlet ground state, which invariably gets masked due to different solid-state effects (e.g. hopping). Here, we try to probe the trueness of the atomic SOC-based proposal in an apparently 1-dimensional system, Sr$_3$NaIrO$_6$, possessing a 2$H$ hexagonal structure with well separated Ir$^{5+}$ (5$d^4$) ions. But all the detailed experimental as well as theoretical characterizations reveal that the ground state of Sr$_3$NaIrO$_6$ is not nonmagnetic, rather accommodating a significantly high effective magnetic moment on Ir$^{5+}$ ion. However our combined dc susceptibility ($χ$), ${}^{23}$Na nuclear magnetic resonance (NMR), muon-spin-relaxation/rotation ($μ$SR) and heat capacity ($C_p$) measurements clearly refute any sign of spin-freezing or ordered magnetism among the Ir$^{5+}$ moments due to geometrical exchange frustration, while in-depth zero-field (ZF) and longitudinal field (LF) $μ$SR investigations strongly point towards inhomogeneous quantum spin-orbital liquid (QSOL)-like ground state. In addition, the linear temperature dependence of both the NMR spin-lattice relaxation rate and the magnetic heat capacity at low temperatures suggest low-lying gapless spin excitations in the QSOL phase of this material. Finally, we conclude that the effective SOC realised in $d^4$ iridates are unlikely to offer a ground state which will be consistent with a purely atomic $j$-$j$ coupling description.

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arXiv2021

Universal fluctuating regime in triangular chromate antiferromagnets

We report x-ray diffraction, magnetic susceptibility, heat capacity, $^{1}$H nuclear magnetic resonance (NMR), and muon spin relaxation ($μ$SR) measurements, as well as density-functional band-structure calculations for the frustrated $S=3/2$ triangular lattice Heisenberg antiferromagnet (TLHAF) $α$-HCrO$_{2}$ (trigonal, space group: $R\bar{3}m$). This compound undergoes a clear magnetic transition at $T_{\rm N} \simeq 22.5$~K, as seen from the drop in the muon paramagnetic fraction and concurrent anomalies in the magnetic susceptibility and specific heat. Local probes (NMR and $μ$SR) reveal a broad regime with slow fluctuations down to $0.7\,T_{\rm N}$, this temperature corresponding to the maximum in the $μ$SR relaxation rate and in the NMR wipe-out. From the comparison with NaCrO$_{2}$ and $α$-KCrO$_{2}$, the fluctuating regime and slow dynamics below $T_{\rm N}$ appear to be hallmarks of the TLHAF with $ABC$ stacking that leads to a frustration of interlayer couplings between the triangular planes. This interlayer frustration is a powerful lever to generate spin states with persistent dynamics and may bear implications to spin-liquid candidates with the triangular geometry.

cond-mat.mtrl-sci↗

arXiv2021

Unusual spin dynamics in the low-temperature magnetically ordered state of Ag$_{3}$LiIr$_{2}$O$_{6}$

Recently, there have been contrary claims of Kitaev spin-liquid behaviour and ordered behavior in the honeycomb compound Ag$_3$LiIr$_2$O$_6$ based on various experimental signatures. Our investigations on this system reveal a low-temperature ordered state with persistent dynamics down to the lowest temperatures. Magnetic order is confirmed by clear oscillations in the muon spin relaxation ($μ$SR) time spectrum below 9 K till 52 mK. Coincidentally in $^7$Li nuclear magnetic resonance, a wipe-out of the signal is observed below $\sim$ 10 K which again strongly indicates magnetic order in the low temperature regime. This is supported by our density functional theory calculations which show an appreciable Heisenberg exchange term in the spin Hamiltonian that favors magnetic ordering. The $^7$Li shift and spin-lattice relaxation rate also show anomalies at $\sim$ 50 K. They are likely related to the onset of dynamic magnetic correlations, but their origin is not completely clear. Detailed analysis of our $μ$SR data is consistent with a co-existence of incommensurate Néel and striped environments. A significant and undiminished dynamical relaxation rate ($\sim 5$ MHz) as seen in $μ$SR deep into the ordered phase indicates enhanced quantum fluctuations in the ordered state.

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arXiv2020

NMR study of magnetic structure and hyperfine interactions in binary helimagnet FeP

We report a detailed study of the ground state helical magnetic structure in monophosphide FeP by means of ${}^{31}$P NMR spectroscopy. We show that the zero-field NMR spectrum of the polycrystalline sample provides strong evidence of an anisotropic distribution of local magnetic fields at the P site with substantially lower anharmonicity than that found at the Fe site by Mössbauer spectroscopy. From field-sweep ${}^{31}$P NMR spectra we conclude that a continuous spin-reorientation transition occurs in an external magnetic field range of 4 - 7 T, which is also confirmed by specific-heat measurements. We observe two pairs of magnetically inequivalent phosphorus positions resulting in a pronounced four-peak structure of the single crystal ${}^{31}$P NMR spectra characteristic of an incommensurate helimagnetic ground state. We revealed a spatial redistribution of local fields at the P sites caused by Fe spin-reorientation transition in high fields and developed an effective approach to account for it. We demonstrate that all observed ${}^{31}$P spectra can be treated within a model of an isotropic helix of Fe magnetic moments in the ($ab$)-plane with a phase shift of 36$^{\circ}$ and 176$^{\circ}$ between Fe1-Fe3 (Fe2-Fe4) and Fe1-Fe2 (Fe3-Fe4) sites, respectively, in accordance with the neutron scattering data.

cond-mat.str-el↗

arXiv2020

Field evolution of low-energy excitations in the hyperhoneycomb magnet $β$-Li$_2$IrO$_3$

$^7$Li nuclear magnetic resonance (NMR) and terahertz (THz) spectroscopies are used to probe magnetic excitations and their field dependence in the hyperhoneycomb Kitaev magnet $β$-Li$_2$IrO$_3$. Spin-lattice relaxation rate ($1/T_1$) measured down to 100\,mK indicates gapless nature of the excitations at low fields (below $H_c\simeq 2.8$\,T), in contrast to the gapped magnon excitations found in the honeycomb Kitaev magnet $α$-RuCl$_3$ at zero applied magnetic field. At higher temperatures in $β$-Li$_2$IrO$_3$, $1/T_1$ passes through a broad maximum without any clear anomaly at the Néel temperature $T_N\simeq 38$\,K, suggesting the abundance of low-energy excitations that are indeed observed as two peaks in the THz spectra, both correspond to zone-center magnon excitations. At higher fields (above $H_c$), an excitation gap opens, and a re-distribution of the THz spectral weight is observed without any indication of an excitation continuum, in contrast to $α$-RuCl$_3$ where an excitation continuum was reported.

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arXiv2019

LiZn$_{2}$V$_{3}$O$_{8}$: A new geometrically frustrated cluster spin-glass

We have investigated the structural and magnetic properties of a new cubic spinel LiZn$_{2}$V$_{3}$O$_{8}$ (LZVO) through x-ray diffraction, dc and ac susceptibility, magnetic relaxation, aging, memory effect, heat capacity and $^{7}$Li nuclear magnetic resonance (NMR) measurements. A Curie-Weiss fit of the dc susceptibility $χ_{\mathrm{dc}}$($\mathit{T}$) yields a Curie-Weiss temperature $\mathrmθ_{\mathrm{CW}}$ = -185 K. This suggests strong antiferromagnetic (AFM) interactions among the magnetic vanadium ions. The dc and ac susceptibility data indicate the spin-glass behavior below a freezing temperature $T_{f}$ $\simeq$ 3 K. The frequency dependence of the $T_{f}$ is characterized by the Vogel-Fulcher law and critical dynamic scaling behavior or power law. From both fitting, we obtained the value of the characteristic angular frequency $ω_{0}$ $\approx$ 3.56$\times$10$^{6}$ Hz, the dynamic exponent $\mathit{zv}$ $\approx$ 2.65, and the critical time constant $τ_{0}$ $\approx$ 1.82$\times$10$^{-6}$ s, which falls in the conventional range for typical cluster spin-glass (CSG) systems. The value of relative shift in freezing temperature $δT_{f}$ $\simeq$ 0.039 supports a CSG ground states. We also found aging phenomena and memory effects in LZVO. The asymmetric response of the magnetic relaxation below $T_{f}$ supports the hierarchical model. Heat capacity data show no long-range or short-range ordering down to 2 K. Only about 25% magnetic entropy change $(ΔS_{\mathrm{m}})$ signifies the presence of strong frustration in the system. The $^{7}$Li NMR spectra show a shift and broadening with decreasing temperature. The spin-lattice and spin-spin relaxation rates show anomalies due to spin freezing around 3 K as the bulk magnetization.

cond-mat.str-el↗

arXiv2019

Anisotropic temperature-field phase diagram of single-crystalline $β$-Li$_2$IrO$_3$: magnetization, specific heat, and $^7$Li NMR study

Detailed magnetization, specific heat, and $^7$Li nuclear magnetic resonance (NMR) measurements on single crystals of the hyperhoneycomb Kitaev magnet $β$-Li$_2$IrO$_3$ are reported. At high temperatures, {\cred anisotropy of the magnetization is reflected by the different Curie-Weiss temperatures for different field directions}, in agreement with the combination of a ferromagnetic Kitaev interaction ($K$) and a negative off-diagonal anisotropy ($Γ$) as two leading terms in the spin Hamiltonian. At low temperatures, magnetic fields applied along $a$ or $c$ have only a weak effect on the system and reduce the Néel temperature from 38 K at 0 T to about 35.5 K at 14 T, with no field-induced transitions observed up to 58 T on a powder sample. In contrast, the field applied along $b$ causes a drastic reduction in the $T_N$ that vanishes around $H_c=2.8$ T giving way to a crossover toward a quantum paramagnetic state. $^7$Li NMR measurements in this field-induced state reveal a gradual line broadening and a continuous evolution of the line shift with temperature, suggesting the development of local magnetic fields. The spin-lattice relaxation rate shows a peak around the crossover temperature 40 K and follows power-law behavior below this temperature.

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arXiv2019

Structural, thermodynamic, and local probe investigations of a honeycomb material Ag$_{3}$LiMn$_{2}$O$_{6}$

The system Ag[Li$_{1/3}$Mn$_{2/3}$]O$_{2}$ belongs to a quaternary 3R-delafossite family and crystallizes in a monoclinic symmetry with space group $C\,2/m$ and the magnetic Mn$^{4+}$($S=3/2$) ions form a honeycomb network in the $ab$-plane. An anomaly around 50 K and the presence of antiferromagnetic (AFM) coupling (Curie-Weiss temperature $θ_{CW}\sim-51$ K) were inferred from our magnetic susceptibility data. The magnetic specific heat clearly manifests the onset of magnetic ordering in the vicinity of 48\,K and the recovered magnetic entropy, above the ordering temperature, falls short of the expected value, implying the presence of short-range magnetic correlations. The (ESR) line broadening on approaching the ordering temperature $T_{\rm N}$ could be described in terms of a Berezinski-Kosterlitz-Thouless (BKT) scenario with $T_{\rm KT}=40(1)$ K. $^{7}$Li NMR line-shift probed as a function of temperature tracks the static susceptibility (K$_{iso}$) of magnetically coupled Mn$^{4+}$ ions. The $^{7}$Li spin-lattice relaxation rate (1/$T$$_{1}$) exhibits a sharp decrease below about 50 K. Combining our bulk and local probe measurements, we establish the presence of an ordered ground state for the honeycomb system Ag$_{3}$LiMn$_{2}$O$_{6}$.Our ab-initio electronic structure calculations suggest that in the $ab$-plane, the nearest neighbor (NN) exchange interaction is strong and AFM, while the next NN and the third NN exchange interactions are FM and AFM respectively. In the absence of any frustration the system is expected to exhibit long-range, AFM order, in agreement with experiment.

cond-mat.str-el↗

arXiv2019

Unconventional magnetism in the 4d$^{4}$ based ($S=1$) honeycomb system Ag$_{3}$LiRu$_{2}$O$_{6}$

We have investigated the thermodynamic and local magnetic properties of the Mott insulating system Ag$_{3}$LiRu$_{2}$O$_{6}$ containing Ru$^{4+}$ (4$d$$^{4}$) for novel magnetism. The material crystallizes in a monoclinic $C2/m$ structure with RuO$_{6}$ octahedra forming an edge-shared two-dimensional honeycomb lattice with limited stacking order along the $c$-direction. The large negative Curie-Weiss temperature ($θ_{CW}$ = -57 K) suggests antiferromagnetic interactions among Ru$^{4+}$ ions though magnetic susceptibility and heat capacity show no indication of magnetic long-range order down to 1.8 K and 0.4 K, respectively. $^{7}$Li nuclear magnetic resonance (NMR) shift follows the bulk susceptibility between 120-300 K and levels off below 120 K. Together with a power-law behavior in the temperature dependent spin-lattice relaxation rate between 0.2 and 2 K, it suggest dynamic spin correlations with gapless excitations. Electronic structure calculations suggest an $S = 1$ description of the Ru-moments and the possible importance of further neighbour interactions as also bi-quadratic and ring-exchange terms in determining the magnetic properties. Analysis of our $μ$SR data indicates spin freezing below 5 K but the spins remain on the borderline between static and dynamic magnetism even at 20 mK.

cond-mat.str-el↗

arXiv2019

Structural and magnetic properties of a new cubic spinel LiRhMnO$_{4}$

We report the structural and magnetic properties of a new system LiRhMnO$_{4}$ (LRMO) through x-ray diffraction, bulk magnetization, heat capacity and $^{7}$Li nuclear magnetic resonance (NMR) measurements. LRMO crystallizes in the cubic space group $\mathit{Fd}$$\bar{3}$$\mathit{m}$. From the DC susceptibility data, we obtained the Curie-Weiss temperature $\mathrmθ_{\mathrm{CW}}$ = -26 K and Curie constant $\mathit{C}$ = 1.79 Kcm$^{3}$/mol suggesting antiferromagnetic correlations among the magnetic Mn$^{4+}$ ions with an effective spin $\mathit{S}$ = $\frac{3}{2}$. At $\mathit{H}$ = 50 Oe, the field cooled and zero-field cooled magnetizations bifurcate at a freezing temperature, $T_{f}$ = 4.45 K, which yields the frustration parameter $\mathit{f=\frac{\midθ_{CW}\mid}{T_{f}}}>$5. AC susceptibility, shows a cusp-like peak at around $T_{f}$, with the peak position shifting as a function of the driving frequency, confirming a spin-glass-like transition in LRMO. LRMO also shows typical spin-glass characteristics such as memory effect, aging effect and relaxation. In the heat capacity, there is no sharp anomaly down to 2 K indicative of long-range ordering. The field sweep $^{7}$Li NMR spectra show broadening with decreasing temperature without any spectral line shift. The $^{7}$Li NMR spin-lattice and spin-spin relaxation rates also show anomalies due to spin freezing near $T_{f}$.

cond-mat.str-el↗

arXiv2018

Exotic phases of frustrated antiferromagnet LiCu2O2

7Li NMR spectra were measured in a magnetic field up to 17 T at temperatures 5-30 K on single crystalline LiCu2O2. Earlier reported anomalies on magnetization curves correspond to magnetic field values where we observe changes of the NMR spectral shape. For the interpretation of the field and temperature evolutions of our NMR spectra, the magnetic structures were analyzed in the frame of the phenomenological theoretical approach of the Dzyaloshinskii-Landau theory. A set of possible planar and collinear structures was obtained. Most of these structures have an unusual configuration; they are characterized by a two-component order parameter and their magnetic moments vary harmonically not only in direction, but also in size. From the modeling of the observed spectra, a possible scenario of magnetic structure transformations is obtained.

cond-mat.str-el↗

arXiv2017

Persistent low-temperature spin dynamics in the mixed-valence iridate Ba$_{3}$InIr$_{2}$O$_{9}$

Using thermodynamic measurements, neutron diffraction, nuclear magnetic resonance, and muon spin relaxation, we establish putative quantum spin-liquid behavior in Ba$_3$InIr$_2$O$_9$, where unpaired electrons are localized on mixed-valence Ir$_2$O$_9$ dimers with Ir$^{4.5+}$ ions. Despite the antiferromagnetic Curie-Weiss temperature on the order of 10 K, neither long-range magnetic order nor spin freezing are observed down to at least 20 mK, such that spins are short-range correlated and dynamic over nearly three decades in temperature. Quadratic power-law behavior of both the spin-lattice relaxation rate and specific heat indicates the gapless nature of the ground state. We envisage that this exotic behavior may be related to an unprecedented combination of the triangular and buckled honeycomb geometries of nearest-neighbor exchange couplings in the mixed-valence setting.

cond-mat.str-el↗

arXiv2014

Search for a spin-nematic phase in the quasi-one-dimensional frustrated magnet LiCuVO$_4$

We have performed NMR experiments on the quasi one-dimensional frustrated spin-1/2 system LiCuVO$_4$ in magnetic fields $H$ applied along the c-axis up to field values near the saturation field $H_{\rm sat}$. For the field range $H_{\rm c2} 41.4$T, indicating that the majority of magnetic moments in LiCuVO$_4$ are already saturated in this field range. This result is inconsistent with the previously observed linear field dependence of the magnetization $M(H)$ for $H_{\rm c3}<H<H_{\rm sat}$ with $μ_0H_{\rm sat}=45$T [L. E. Svistov {\it et al}., JETP Letters {\bf 93}, 21 (2011)]. We argue that the discrepancy is due to non-magnetic defects in the samples. The results of the spin-lattice relaxation rate of $^7$Li nuclei indicate an energy gap which grows with field twice as fast as the Zeeman energy of a single spin, therefore, suggesting that the two-magnon bound state is the lowest energy excitation. The energy gap tends to close at $μ_0H \approx 41$T. Our results suggest that the theoretically predicted spin-nematic phase, if it exists in LiCuVO$_4$, can be established only within the narrow field range $40.5 < μ_0 H < 41.4$T .

cond-mat.mtrl-sci↗

arXiv2013

Interplay between localized and itinerant magnetism in Co substituted FeGa$_3$

The evolution of the electronic structure and magnetic properties with Co substitution for Fe in the solid solution Fe$_{1-x}$Co$_x$Ga$_3$ was studied by means of electrical resistivity, magnetization, ab-initio band structure calculations, and nuclear spin-lattice relaxation $1/T_1$ of the $^{69,71}$Ga nuclei. Temperature dependencies of the electrical resistivity reveal that the evolution from the semiconducting to the metallic state in the Fe$_{1-x}$Co$_x$Ga$_3$ system occurs at $0.025<x<0.075$. The $^{69,71}(1/T_1)$ was studied as a function of temperature in a wide temperature range of $2\!-\!300$ K for the concentrations $x = 0.0,$ $0.5,$ and $1.0$. In the parent semiconducting compound FeGa$_3$, the temperature dependence of the $^{69}(1/T_1)$ exhibits a huge maximum at about $T\!\sim\!6$ K indicating the existence of in-gap states. The opposite binary compound, CoGa$_3$, demonstrates a metallic Korringa behavior with $1/T_1$ $\propto T$. In Fe$_{0.5}$Co$_{0.5}$Ga$_3$, the relaxation is strongly enhanced due to spin fluctuations and follows $1/T_1\propto T^{1/2}$, which is a unique feature of weakly and nearly antiferromagnetic metals. This itinerant antiferromagnetic behavior contrasts with both magnetization measurements, showing localized magnetism with a relatively low effective moment of about 0.7 $μ_B$/f.u., and ab initio band structure calculations, where a ferromagnetic state with an ordered moment of 0.5 $μ_B$/f.u. is predicted. The results are discussed in terms of the interplay betwen the localized and itinerant magnetizm including in-gap states and spin fluctuations.

cond-mat.mtrl-sci↗

arXiv2013

Magnetic structure of the frustrated S=1/2 chain magnet LiCu2O2 doped with nonmagnetic Zn

We present the results of magnetization, ESR and NMR measurements on single crystal samples of the frustrated S=1/2 chain cuprate LiCu2O2 doped with nonmagnetic Zn^2+. As shown by the x-ray techniques the crystals of Li(Cu{1-x}Zn{x})2O2 with x<0.12 are single-phase, whereas for higher Zn concentrations the samples were polyphase. ESR spectra for all monophase samples (0<= x<0.12) can be explained within the model of a planar spin structure with a uniaxial type anisotropy. The NMR spectra of the highly doped single crystal sample Li(Cu0.9Zn0.1)2O2 can be described in the frame of a planar spin glass like magnetic structure with short range spiral correlations in the crystal (ab)-planes with strongest exchange bonds. The value of magnetic moments of Cu^2+ ions in this structure is close to value obtained for undoped crystals: (0.8 +- 0.1) mu_B.

cond-mat.str-el↗

arXiv2009

Intermediate-valence behavior of the transition-metal oxide CaCu$_3$Ru$_4$O$_{12}$

The transition--metal oxide CaCu$_3$Ru$_4$O$_{12}$ with perovskite--type structure shows characteristic properties of an intermediate--valence system. The temperature--dependent susceptibility exhibits a broad maximum around $150 - 160$ K. At this temperature, neutron powder diffraction reveals a small but significant volume change whereby the crystal structure is preserved. Moreover, the temperature--dependent resistivity changes its slope. NMR Knight shift measurements of Ru reveal a cross--over from high temperature paramagnetic behavior of localized moments to itinerant band states at low temperatures. Additional density--functional theory calculations can relate the structural anomaly with the $d$--electron number. The different experimental and calculational methods result in a mutually consistent description of CaCu$_3$Ru$_4$O$_{12}$ as an intermediate--valent system in the classical sense of having low--energy charge fluctuations.

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